TY - JOUR
T1 - In Situ Characterizations Revealing Ruthenium-Atom-Induced Raise of Photocatalytic Performance
AU - Talebian-Kiakalaieh, Amin
AU - Guo, Meijun
AU - Hashem, Elhussein M.
AU - Xia, Bingquan
AU - Jiang, Yunling
AU - Chuah, Clarence
AU - Tang, Youhong
AU - Kwong, Philip
AU - Ran, Jingrun
AU - Qiao, Shi Zhang
PY - 2023/10/6
Y1 - 2023/10/6
N2 - Rational design/fabrication of high-activity photocatalysts is of central importance to realize solar-to-chemical conversion for tackling worldwide energy/environmental issues. Hence, it is desirable to disclose the element/space/time-resolved charge kinetics and surface species evolution of photocatalysts under realistic conditions using various in situ characterizations. Furthermore, the correlation of the above-disclosed mechanisms with atomic-scale compositions/structures of photocatalysts can further direct the atomic-level design/synthesis of high-performance photocatalysts. Herein, Ru atoms incorporated CdS quantum dots (QDs) are synthesized using an in situ hot-injection route. The optimized Ru incorporated CdS QDs (Ru0.1) exhibit excellent photocatalytic evolution rates of H2O2 (8.78 mmol g−1 h−1) and benzaldehyde (11.70 mmol g−1 h−1), respectively. Four different in situ characterizations demonstrate that in realistic conditions, the incorporated Ru atoms with high oxidation state (+3) effectively attract photo-generated electrons from bulk to the overall surface of Ru0.1; these directed electron flows also greatly facilitate the transfer of photo-generated holes from bulk to surface of Ru0.1 via efficiently reducing electron-hole recombination. in situ diffuse reflectance infrared Fourier transform spectroscopy, electron spin spectroscopy, and species-trapping experiments further reveal three possible reaction pathways for H2O2 evolution. This work underscores the use of in situ characterizations to reveal the element/space/time-resolved electrons/holes kinetics and surface-species generation for photocatalysts in realistic conditions.
AB - Rational design/fabrication of high-activity photocatalysts is of central importance to realize solar-to-chemical conversion for tackling worldwide energy/environmental issues. Hence, it is desirable to disclose the element/space/time-resolved charge kinetics and surface species evolution of photocatalysts under realistic conditions using various in situ characterizations. Furthermore, the correlation of the above-disclosed mechanisms with atomic-scale compositions/structures of photocatalysts can further direct the atomic-level design/synthesis of high-performance photocatalysts. Herein, Ru atoms incorporated CdS quantum dots (QDs) are synthesized using an in situ hot-injection route. The optimized Ru incorporated CdS QDs (Ru0.1) exhibit excellent photocatalytic evolution rates of H2O2 (8.78 mmol g−1 h−1) and benzaldehyde (11.70 mmol g−1 h−1), respectively. Four different in situ characterizations demonstrate that in realistic conditions, the incorporated Ru atoms with high oxidation state (+3) effectively attract photo-generated electrons from bulk to the overall surface of Ru0.1; these directed electron flows also greatly facilitate the transfer of photo-generated holes from bulk to surface of Ru0.1 via efficiently reducing electron-hole recombination. in situ diffuse reflectance infrared Fourier transform spectroscopy, electron spin spectroscopy, and species-trapping experiments further reveal three possible reaction pathways for H2O2 evolution. This work underscores the use of in situ characterizations to reveal the element/space/time-resolved electrons/holes kinetics and surface-species generation for photocatalysts in realistic conditions.
KW - HO evolution
KW - in situ characterizations
KW - realistic charge kinetics
KW - Ru atoms
UR - http://www.scopus.com/inward/record.url?scp=85167463405&partnerID=8YFLogxK
UR - http://purl.org/au-research/grants/ARC/FL170100154
UR - http://purl.org/au-research/grants/ARC/DE200100629
UR - http://purl.org/au-research/grants/ARC/DP22102596
UR - http://purl.org/au-research/grants/ARC/LP210301397
UR - http://purl.org/au-research/grants/ARC/CE230100032
U2 - 10.1002/aenm.202301594
DO - 10.1002/aenm.202301594
M3 - Article
AN - SCOPUS:85167463405
SN - 1614-6832
VL - 13
JO - Advanced Energy Materials
JF - Advanced Energy Materials
IS - 37
M1 - 2301594
ER -